The CLAW hypothesis argues that a negative feedback mechanism involving phytoplankton-derived dimethylsulfoniopropionate (DMSP) could mitigate increasing sea surface temperatures that result from global warming. DMSP is converted to the climatically active dimethylsulfide (DMS), which is transferred to the atmosphere and photochemically oxidized to sulfate aerosols, leading to increases in planetary albedo and cooling of the Earth’s atmosphere. A shipboard incubation experiment was conducted to investigate the effects of increased temperature and pCO2 on the algal community structure of the North Atlantic spring bloom and their subsequent impact on particulate and dissolved DMSP concentrations (DMSPp and DMSPd). Under ‘greenhouse’ conditions (elevated pCO2; 690 ppm) and elevated temperature (ambient + 4°C), coccolithophorid and pelagophyte abundances were significantly higher than under control conditions (390 ppm CO2 and ambient temperature). This shift in phytoplankton community structure also resulted in an increase in DMSPp concentrations and DMSPp:chl a ratios. There were also increases in DMSP-lyase activity and biomass-normalized DMSP-lyase activity under ‘greenhouse’ conditions. Concentrations of DMSPd decreased in the ‘greenhouse’ treatment relative to the control. This decline is thought to be partly due to changes in the microzooplankton community structure and decreased grazing pressure under ‘greenhouse’ conditions. The increases in DMSPp in the high temperature and greenhouse treatments support the CLAW hypothesis; the declines in DMSPd do not.